{"title":"理论-界面协同设计实现高效电催化和能量存储的多功能电极","authors":"Min Zhu, , , Xuerong Shi*, , , Shengming Zhang, , , Xinlei Yu, , , Runlin Wang, , , Peijie Wang, , , Rujing Shang*, , and , Shusheng Xu*, ","doi":"10.1021/acs.langmuir.5c03303","DOIUrl":null,"url":null,"abstract":"<p >The strategic design of integrated catalysts for overall water splitting, urea electrolysis, and energy storage represents an unexplored frontier with significant challenges for catalyst engineering. Inspired by theoretical predictions that CoP/CoNi<sub>2</sub>S<sub>4</sub> composites exhibit enhanced hydrogen evolution reaction (HER) activity compared to individual components, this nanorod structure was fabricated, demonstrating exceptional HER performance across acidic, alkaline, and simulated seawater conditions. It achieved 10 mA cm<sup>–2</sup> at overpotentials of 119 mV (acidic), 88 mV (alkaline), and 95 mV (seawater), with 100-h stability, surpassing commercial Pt/C at high current densities (200 mA cm<sup>–2</sup>) with η<sub>200</sub> values of 232 mV (1 M KOH) and 234 mV (1 M KOH + 0.5 M NaCl). For oxygen evolution reaction (OER), it exhibited superior activity in alkaline media (η<sub>10</sub> = 267 mV) and simulated seawater, outperforming commercial RuO<sub>2</sub>. In urea-added electrolytes, the symmetric electrolyzer required only 1.53 V to achieve 10 mA cm<sup>–2</sup>. As a hybrid supercapacitor, the assembled CoP/CoNi<sub>2</sub>S<sub>4</sub>//AC device delivered an energy density of 50.9 Wh kg<sup>–1</sup> at 800 W kg<sup>–1</sup> with excellent cycling stability. This TMP/TMS composite integrates electrocatalytic and energy storage functionalities, paving the way for multifunctional applications in energy conversion technologies.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"41 38","pages":"26276–26289"},"PeriodicalIF":3.9000,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Theoretical-Interfacial Codesign Enabling a Multi-Functional Electrode for Efficient Electrocatalysis and Energy Storage\",\"authors\":\"Min Zhu, , , Xuerong Shi*, , , Shengming Zhang, , , Xinlei Yu, , , Runlin Wang, , , Peijie Wang, , , Rujing Shang*, , and , Shusheng Xu*, \",\"doi\":\"10.1021/acs.langmuir.5c03303\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The strategic design of integrated catalysts for overall water splitting, urea electrolysis, and energy storage represents an unexplored frontier with significant challenges for catalyst engineering. Inspired by theoretical predictions that CoP/CoNi<sub>2</sub>S<sub>4</sub> composites exhibit enhanced hydrogen evolution reaction (HER) activity compared to individual components, this nanorod structure was fabricated, demonstrating exceptional HER performance across acidic, alkaline, and simulated seawater conditions. It achieved 10 mA cm<sup>–2</sup> at overpotentials of 119 mV (acidic), 88 mV (alkaline), and 95 mV (seawater), with 100-h stability, surpassing commercial Pt/C at high current densities (200 mA cm<sup>–2</sup>) with η<sub>200</sub> values of 232 mV (1 M KOH) and 234 mV (1 M KOH + 0.5 M NaCl). For oxygen evolution reaction (OER), it exhibited superior activity in alkaline media (η<sub>10</sub> = 267 mV) and simulated seawater, outperforming commercial RuO<sub>2</sub>. In urea-added electrolytes, the symmetric electrolyzer required only 1.53 V to achieve 10 mA cm<sup>–2</sup>. As a hybrid supercapacitor, the assembled CoP/CoNi<sub>2</sub>S<sub>4</sub>//AC device delivered an energy density of 50.9 Wh kg<sup>–1</sup> at 800 W kg<sup>–1</sup> with excellent cycling stability. This TMP/TMS composite integrates electrocatalytic and energy storage functionalities, paving the way for multifunctional applications in energy conversion technologies.</p>\",\"PeriodicalId\":50,\"journal\":{\"name\":\"Langmuir\",\"volume\":\"41 38\",\"pages\":\"26276–26289\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-09-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Langmuir\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.langmuir.5c03303\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Langmuir","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.langmuir.5c03303","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
整体水分解、尿素电解和储能一体化催化剂的战略设计是催化剂工程中一个未开发的前沿领域，具有重大挑战。CoP/CoNi2S4复合材料的理论预测表明，与单个组分相比，其析氢反应（HER）活性增强。受此理论预测的启发，该纳米棒结构在酸性、碱性和模拟海水条件下都表现出优异的析氢反应性能。在过电位为119 mV（酸性）、88 mV（碱性）和95 mV（海水）的情况下，它的稳定性为10 mA cm-2，在高电流密度（200 mA cm-2）下，η值分别为232 mV （1 M KOH）和234 mV (1 M KOH + 0.5 M NaCl)，其稳定性超过了商用Pt/C。在碱性介质（η10 = 267 mV）和模拟海水中表现出更强的析氧活性，优于商用RuO2。在添加尿素的电解质中，对称电解槽只需要1.53 V就能达到10 mA cm-2。作为一种混合超级电容器，组装的CoP/CoNi2S4//AC器件在800 W kg-1时的能量密度为50.9 Wh kg-1，具有良好的循环稳定性。这种TMP/TMS复合材料集成了电催化和能量存储功能，为能量转换技术的多功能应用铺平了道路。
Theoretical-Interfacial Codesign Enabling a Multi-Functional Electrode for Efficient Electrocatalysis and Energy Storage
The strategic design of integrated catalysts for overall water splitting, urea electrolysis, and energy storage represents an unexplored frontier with significant challenges for catalyst engineering. Inspired by theoretical predictions that CoP/CoNi2S4 composites exhibit enhanced hydrogen evolution reaction (HER) activity compared to individual components, this nanorod structure was fabricated, demonstrating exceptional HER performance across acidic, alkaline, and simulated seawater conditions. It achieved 10 mA cm–2 at overpotentials of 119 mV (acidic), 88 mV (alkaline), and 95 mV (seawater), with 100-h stability, surpassing commercial Pt/C at high current densities (200 mA cm–2) with η200 values of 232 mV (1 M KOH) and 234 mV (1 M KOH + 0.5 M NaCl). For oxygen evolution reaction (OER), it exhibited superior activity in alkaline media (η10 = 267 mV) and simulated seawater, outperforming commercial RuO2. In urea-added electrolytes, the symmetric electrolyzer required only 1.53 V to achieve 10 mA cm–2. As a hybrid supercapacitor, the assembled CoP/CoNi2S4//AC device delivered an energy density of 50.9 Wh kg–1 at 800 W kg–1 with excellent cycling stability. This TMP/TMS composite integrates electrocatalytic and energy storage functionalities, paving the way for multifunctional applications in energy conversion technologies.
期刊介绍：
Langmuir is an interdisciplinary journal publishing articles in the following subject categories:
Colloids: surfactants and self-assembly, dispersions, emulsions, foams
Interfaces: adsorption, reactions, films, forces
Biological Interfaces: biocolloids, biomolecular and biomimetic materials
Materials: nano- and mesostructured materials, polymers, gels, liquid crystals
Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry
Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals
However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do?
Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*.
This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).
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